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优化Ru/WO金属/类金属异质结构电催化剂上的氢和羟基吸附,以在碱性介质中实现高效稳定的氢氧化反应。

Optimizing Hydrogen and Hydroxyl Adsorption over Ru/WO Metal/Metalloid Heterostructure Electrocatalysts for Highly Efficient and Stable Hydrogen Oxidation Reactions in Alkaline Media.

作者信息

Cheng Zhiyu, Yang Yang, Wang Peichen, Wang Pengcheng, Yang Jiahe, Wang Dongdong, Chen Qianwang

机构信息

Hefei National Research Center for Physical Sciences at the Microscale and Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China.

The High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei, 230031, China.

出版信息

Small. 2024 Apr;20(17):e2307780. doi: 10.1002/smll.202307780. Epub 2024 Jan 3.

DOI:10.1002/smll.202307780
PMID:38168535
Abstract

The development of high-performance, stable and platinum-free electrocatalysts for the hydrogen oxidation reaction (HOR) in alkaline media is crucial for the commercial application of anion exchange membrane fuel cells (AEMFCs). Ruthenium, as an emerging HOR electrocatalyst with a price advantage over platinum, still needs to solve the problems of low intrinsic activity and easy oxidation. Herein, Ru nanoparticles are anchored on the oxygen-vacancy-rich metalloid WO by interfacial engineering to create abundant and efficient Ru and WO interfacial active sites for accelerated HOR in alkaline media. Ru/WO/C displays excellent catalytic activity with mass activity (8.29 A mg ) and specific activity (1.32 mA cm ), which are 2.5/3.3 and 21.8/8.3 times that of PtRu/C and Pt/C, respectively. Moreover, Ru/WO/C exhibits excellent CO tolerance and operational stability. Experimental and theoretical studies reveal that the improved charge transfer from Ru to WO in the metal/metalloid heterostructure significantly tune the electronic structure of Ru sites and optimize the hydrogen binding energy (HBE) of Ru. While, WO provides abundant hydroxyl adsorption sites. Therefore, the equilibrium adsorption of hydrogen and hydroxyl at the interface of Ru/WO will be realized, and the oxidation of metal Ru would be avoided, thereby achieving excellent HOR activity and durability.

摘要

开发用于碱性介质中氢氧化反应(HOR)的高性能、稳定且无铂的电催化剂对于阴离子交换膜燃料电池(AEMFC)的商业应用至关重要。钌作为一种新兴的HOR电催化剂,相对于铂具有价格优势,但仍需解决本征活性低和易氧化的问题。在此,通过界面工程将钌纳米颗粒锚定在富含氧空位的类金属WO上,以创建丰富且高效的Ru-WO界面活性位点,用于加速碱性介质中的HOR。Ru/WO/C表现出优异的催化活性,质量活性(8.29 A mg)和比活性(1.32 mA cm)分别是PtRu/C和Pt/C的2.5/3.3倍和21.8/8.3倍。此外,Ru/WO/C表现出优异的CO耐受性和操作稳定性。实验和理论研究表明,金属/类金属异质结构中从Ru到WO的电荷转移改善,显著调节了Ru位点的电子结构并优化了Ru的氢结合能(HBE)。同时,WO提供了丰富的羟基吸附位点。因此,将实现Ru/WO界面处氢和羟基的平衡吸附,避免金属Ru的氧化,从而实现优异的HOR活性和耐久性。

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